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To perform the electrochemical nitrogen reduction reaction (NRR) under milder conditions for sustainable ammonia production, electrocatalysts should exhibit high selectivity, activity, and durability. However, the key restrictions are the highly stable N≡N triple bond and the competitive hydrogen evolution reaction (HER), which make it difficult to adsorb and activate N2 on the surface of electrocatalysts, leading to a low ammonia yield and Faraday efficiency. Inspired by the enzymatic nitrogenase process and using the Fe-Mo as the active center, here we report supported Fe2Mo3O8/XC-72 as an effective and durable electrocatalyst for the NRR. Fe2Mo3O8/XC-72 exhibited NRR activity with an NH3 yield of 30.4 μg·h−1·mg−1 (−0.3 V) and a Faraday efficiency of 8.2% (−0.3 V). Theoretical calculations demonstrated that the electrocatalytic nitrogen fixation mechanism involved the Fe atom in the Fe2Mo3O8/XC-72 electrocatalyst acting as the main active site in the enzymatic pathway (*NH2 → *NH3), which activated nitrogen molecules and promoted the NRR performance.
We acknowledge financial support from the Beijing Municipal High Level Innovative Team Building Program (No. IDHT20180504), Beijing Outstanding Young Scientist Program (No. BJJWZYJH01201910005017), the National Natural Science Foundation of China (Nos. 51801006, 21805004, 21872001, and 21936001), Beijing Natural Science Foundation (No. 2192005), and Beijing Municipal Science and Natural Science Fund Project (Nos. KM201910005016 and 2017000020124G085).